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Complex <jats:bold>1<\/jats:bold> displayed reactivity towards CS<jats:sub>2<\/jats:sub> and CO<jats:sub>2<\/jats:sub> at room temperature that is unprecedented in f\u2010element chemistry, affording diverse N\u2010functionalized products depending on the reaction stoichiometry. The reaction of <jats:bold>1<\/jats:bold> with two equivalents of CS<jats:sub>2<\/jats:sub> yielded the thiocyanate\/thiocarbonate complex Cs{(\u03bc\u2010NCS)(\u03bc\u2010CS<jats:sub>3<\/jats:sub>)[U(OSi(O<jats:sup>t<\/jats:sup>Bu)<jats:sub>3<\/jats:sub>)<jats:sub>3<\/jats:sub>]<jats:sub>2<\/jats:sub>} via a putative NCS<jats:sup>\u2212<\/jats:sup>\/S<jats:sup>2\u2212<\/jats:sup> intermediate. The reaction of <jats:bold>1<\/jats:bold> with one equivalent of CO<jats:sub>2<\/jats:sub> resulted in deoxygenation and N\u2212C bond formation, yielding the cyanate\/oxo complex Cs{(\u03bc\u2010NCO)(\u03bc\u2010O)[U(OSi(O<jats:sup>t<\/jats:sup>Bu)<jats:sub>3<\/jats:sub>)<jats:sub>3<\/jats:sub>]<jats:sub>2<\/jats:sub>}. Addition of excess CO<jats:sub>2<\/jats:sub> to <jats:bold>1<\/jats:bold> led to the unprecedented dicarbamate product Cs{(\u03bc\u2010NC<jats:sub>2<\/jats:sub>O<jats:sub>4<\/jats:sub>)[U(OSi(O<jats:sup>t<\/jats:sup>Bu)<jats:sub>3<\/jats:sub>)<jats:sub>3<\/jats:sub>]<jats:sub>2<\/jats:sub>}.<\/jats:p>","DOI":"10.1002\/anie.201600158","type":"journal-article","created":{"date-parts":[[2016,2,26]],"date-time":"2016-02-26T03:14:09Z","timestamp":1456456449000},"page":"4074-4078","source":"Crossref","is-referenced-by-count":56,"title":["Nucleophilic Reactivity of a Nitride\u2010Bridged Diuranium(IV) Complex: CO<sub>2<\/sub> and CS<sub>2<\/sub> Functionalization"],"prefix":"10.1002","volume":"55","author":[{"given":"Marta","family":"Falcone","sequence":"first","affiliation":[{"name":"Institut des Sciences et Ing\u00e9nierie Chimiques Ecole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL)  1015 Lausanne Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lucile","family":"Chatelain","sequence":"additional","affiliation":[{"name":"Institut des Sciences et Ing\u00e9nierie Chimiques Ecole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL)  1015 Lausanne Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Marinella","family":"Mazzanti","sequence":"additional","affiliation":[{"name":"Institut des Sciences et Ing\u00e9nierie Chimiques Ecole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL)  1015 Lausanne Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2016,2,23]]},"reference":[{"key":"e_1_2_2_1_1","unstructured":"\u00a0"},{"key":"e_1_2_2_2_2","unstructured":"F.Haber DE 229126 1909;"},{"key":"e_1_2_2_3_2","doi-asserted-by":"publisher","DOI":"10.1038\/nature07372"},{"key":"e_1_2_2_4_2","doi-asserted-by":"publisher","DOI":"10.1007\/978-3-642-12073-2_7"},{"key":"e_1_2_2_5_1","unstructured":"\u00a0"},{"key":"e_1_2_2_6_2","doi-asserted-by":"publisher","DOI":"10.1021\/ic901165j"},{"key":"e_1_2_2_7_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2013.06.013"},{"key":"e_1_2_2_8_1","unstructured":"\u00a0"},{"key":"e_1_2_2_9_2","doi-asserted-by":"publisher","DOI":"10.1039\/c3cc39053e"},{"key":"e_1_2_2_10_2","doi-asserted-by":"publisher","DOI":"10.1126\/science.1116452"},{"key":"e_1_2_2_11_2","doi-asserted-by":"publisher","DOI":"10.1002\/1521-3773(20020916)41:18<3433::AID-ANIE3433>3.0.CO;2-V"},{"key":"e_1_2_2_11_3","doi-asserted-by":"publisher","DOI":"10.1002\/1521-3757(20020916)114:18<3583::AID-ANGE3583>3.0.CO;2-B"},{"key":"e_1_2_2_12_2","doi-asserted-by":"publisher","DOI":"10.1021\/ja103588w"},{"key":"e_1_2_2_13_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.200705742"},{"key":"e_1_2_2_13_3","doi-asserted-by":"publisher","DOI":"10.1002\/ange.200705742"},{"key":"e_1_2_2_14_2","doi-asserted-by":"publisher","DOI":"10.1021\/ja101567h"},{"key":"e_1_2_2_15_2","doi-asserted-by":"publisher","DOI":"10.1021\/ja910364u"},{"key":"e_1_2_2_16_2","doi-asserted-by":"publisher","DOI":"10.1021\/ja405815b"},{"key":"e_1_2_2_17_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.inorgchem.5b01547"},{"key":"e_1_2_2_18_2","doi-asserted-by":"publisher","DOI":"10.1038\/nchem.705"},{"key":"e_1_2_2_19_2","doi-asserted-by":"publisher","DOI":"10.1038\/nchem.1642"},{"key":"e_1_2_2_20_2","doi-asserted-by":"publisher","DOI":"10.1126\/science.1223488"},{"key":"e_1_2_2_21_2","doi-asserted-by":"publisher","DOI":"10.1021\/ja502405e"},{"key":"e_1_2_2_22_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201406203"},{"key":"e_1_2_2_22_3","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201406203"},{"key":"e_1_2_2_23_1","doi-asserted-by":"publisher","DOI":"10.1021\/jm200187y"},{"key":"e_1_2_2_24_1","doi-asserted-by":"publisher","DOI":"10.1039\/b700658f"},{"key":"e_1_2_2_25_1","unstructured":"\u00a0"},{"key":"e_1_2_2_26_2","doi-asserted-by":"publisher","DOI":"10.1021\/ja405477m"},{"key":"e_1_2_2_27_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201307097"},{"key":"e_1_2_2_27_3","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201307097"},{"key":"e_1_2_2_28_1","unstructured":"\u00a0"},{"key":"e_1_2_2_29_2","doi-asserted-by":"publisher","DOI":"10.1002\/9781118792797.ch06"},{"key":"e_1_2_2_30_2","doi-asserted-by":"publisher","DOI":"10.1039\/b111550m"},{"key":"e_1_2_2_31_2","doi-asserted-by":"publisher","DOI":"10.1021\/ja910445r"},{"key":"e_1_2_2_32_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201307291"},{"key":"e_1_2_2_32_2","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201307291"},{"key":"e_1_2_2_33_1","unstructured":"\u00a0"},{"key":"e_1_2_2_34_2","doi-asserted-by":"publisher","DOI":"10.1021\/ja00222a011"},{"key":"e_1_2_2_35_2","first-page":"587","volume":"19","author":"Stewart J. 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